Detection, Quantification, and Isomer Differentiation of Per- and Polyfluoroalkyl Substances (PFAS) Using MALDI-TOF with Trapped Ion Mobility

January 22, 2024 - Aidan J. Reynolds, Abby M. Smith and Tian Autumn Qiu

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Abstract

Per- and polyfluoroalkyl substances (PFAS) are a class of organic compounds that have attracted global attention for their persistence in the environment, exposure to biological organisms, and their adverse health effects. There is an urgent need to develop analytical methodologies for the characterization of PFAS in various sample matrices. Matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) represents a chromatography-free MS method that performs laser-based ionization and in situ analysis on samples. In this study, we present PFAS analysis by MALDI-time-of-flight (TOF) MS with trapped ion mobility spectrometry (TIMS), which provides an additional dimension of gas phase separation based on the size-to-charge ratios. MALDI matrix composition and key instrument parameters were optimized to produce different ranges of calibration curves. Parts per billion (ppb) range of calibration curves were achieved for a list of legacy and alternative perfluorosulfonic acids (PFSAs) and perfluorocarboxylic acids (PFCAs), while ion mobility spectrum filtering enabled parts per trillion (ppt) range of calibration curves for PFSAs. We also successfully demonstrated the separation of three perfluorooctanesulfonic acid (PFOS) structural isomers in the gas phase using TIMS. Our results demonstrated the new development of utilizing MALDI-TOF-MS coupled with TIMS for fast, quantitative, and sensitive analysis of PFAS, paving ways to future high-throughput and in situ analysis of PFAS such as MS imaging applications.

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